Sequence-dependent structure/function relationships of catalytic peptide-enabled gold nanoparticles generated under ambient synthetic conditions Bedford, Nicholas M., Hughes, Zak E., Tang, Zhenghua, Li, Yue, Briggs, Beverly D., Ren, Yang, Swihart, Mark T., Petkov, Valeri G., Naik, Rajesh R., Knecht, Marc R. and Walsh,Tiffany R. 2016, Sequence-dependent structure/function relationships of catalytic peptide-enabled gold nanoparticles generated under ambient synthetic conditions, Journal of the American chemistry society, vol. 138, no. 2, pp. 540-548, doi: 10.1021/jacs.5b09529. Attached Files Name Description MIMEType Size Downloads Title Sequence-dependent structure/function relationships of catalytic peptide-enabled gold nanoparticles generated under ambient synthetic conditions Author(s) Bedford, Nicholas M. Hughes, Zak E. orcid.org/0000-0003-2166-9822 Tang, Zhenghua Li, Yue Briggs, Beverly D. Ren, Yang Swihart, Mark T. Petkov, Valeri G. Naik, Rajesh R. Knecht, Marc R. Walsh,Tiffany R. orcid.org/0000-0002-0233-9484 Journal name Journal of the American chemistry society Volume number 138 Issue number 2 Start page 540 End page 548 Total pages 9 Publisher ACS Publications Place of publication Washington, D.C. Publication date 2016 ISSN 1520-5126 Keyword(s) Science & Technology Physical Sciences Chemistry, Multidisciplinary Chemistry MONTE-CARLO-SIMULATION X-RAY-DIFFRACTION BINDING PEPTIDES NANOMATERIAL SYNTHESIS BIOMIMETIC SYNTHESIS ADSORPTION BEHAVIOR MEDIATED SYNTHESIS REPLICA EXCHANGE AQUEOUS-SOLUTION RECOGNITION Summary Peptide-enabled nanoparticle (NP) synthesis routes can create and/or assemble functional nanomaterials under environmentally friendly conditions, with properties dictated by complex interactions at the biotic/abiotic interface. Manipulation of this interface through sequence modification can provide the capability for material properties to be tailored to create enhanced materials for energy, catalysis, and sensing applications. Fully realizing the potential of these materials requires a comprehensive understanding of sequence-dependent structure/function relationships that is presently lacking. In this work, the atomic-scale structures of a series of peptide-capped Au NPs are determined using a combination of atomic pair distribution function analysis of high-energy X-ray diffraction data and advanced molecular dynamics (MD) simulations. The Au NPs produced with different peptide sequences exhibit varying degrees of catalytic activity for the exemplar reaction 4-nitrophenol reduction. The experimentally derived atomic-scale NP configurations reveal sequence-dependent differences in structural order at the NP surface. Replica exchange with solute-tempering MD simulations are then used to predict the morphology of the peptide overlayer on these Au NPs and identify factors determining the structure/catalytic properties relationship. We show that the amount of exposed Au surface, the underlying surface structural disorder, and the interaction strength of the peptide with the Au surface all influence catalytic performance. A simplified computational prediction of catalytic performance is developed that can potentially serve as a screening tool for future studies. Our approach provides a platform for broadening the analysis of catalytic peptide-enabled metallic NP systems, potentially allowing for the development of rational design rules for property enhancement. Language eng DOI 10.1021/jacs.5b09529 Field of Research 030302 Nanochemistry and Supramolecular Chemistry 030601 Catalysis and Mechanisms of Reactions 030406 Proteins and Peptides 030603 Colloid and Surface Chemistry 030704 Statistical Mechanics in Chemistry 03 Chemical Sciences Socio Economic Objective 970103 Expanding Knowledge in the Chemical Sciences HERDC Research category C1 Refereed article in a scholarly journal ERA Research output type C Journal article Copyright notice ©2016, ACS Publications Persistent URL http://hdl.handle.net/10536/DRO/DU:30081011 Document type: Journal Article Collection: Institute for Frontier Materials Related Links Link Description Link Go to link with your DU access privileges   Connect to published version Go to link with your DU access privileges     Unless expressly stated otherwise, the copyright for items in DRO is owned by the author, with all rights reserved. Versions Version Filter Type Fri, 29 Jan 2016, 08:21:40 EST Mon, 18 Apr 2016, 10:57:57 EST Mon, 18 Apr 2016, 12:45:20 EST Mon, 18 Apr 2016, 13:24:54 EST Mon, 18 Apr 2016, 13:34:02 EST Fri, 20 May 2016, 12:10:50 EST Fri, 20 May 2016, 12:12:05 EST Tue, 13 Feb 2018, 07:36:36 EST Filtered Full Citation counts:   Cited 26 times in TR Web of Science Cited 25 times in Scopus Search Google Scholar Access Statistics: 159 Abstract Views, 2 File Downloads  -  Detailed Statistics Created: Mon, 18 Apr 2016, 10:57:57 EST

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